A new method for evaluating regional air quality forecasts

A Kriging interpolation method is combined with an object-based evaluation measure to assess the ability of the UK Met Office's dispersion and weather prediction models to predict the evolution of a plume of tracer as it was transported across Europe. The object-based evaluation method, SAL, considers aspects of the Structure, Amplitude and Location of the pollutant field. The SAL method is able to quantify errors in the predicted size and shape of the pollutant plume, through the structure component, the over- or under-prediction of the pollutant concentrations, through the amplitude component, and the position of the pollutant plume, through the location component. The quantitative results of the SAL evaluation are similar for both models and close to a subjective visual inspection of the predictions. A negative structure component for both models, throughout the entire 60 hour plume dispersion simulation, indicates that the modelled plumes are too small and/or too peaked compared to the observed plume at all times. The amplitude component for both models is strongly positive at the start of the simulation, indicating that surface concentrations are over-predicted by both models for the first 24 hours, but modelled concentrations are within a factor of 2 of the observations at later times. Finally, for both models, the location component is small for the first 48 hours after the start of the tracer release, indicating that the modelled plumes are situated close to the observed plume early on in the simulation, but this plume location error grows at later times. The SAL methodology has also been used to identify differences in the transport of pollution in the dispersion and weather prediction models. The convection scheme in the weather prediction model is found to transport more pollution vertically out of the boundary layer into the free troposphere than the dispersion model convection scheme resulting in lower pollutant concentrations near the surface and hence a better forecast for this case study.

Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn

The budgets of seven halogenated gases (CFC-11, CFC-12, CFC-113, CFC-114, CFC-115, CCl4 and SF6) are studied by comparing measurements in polar firn air from two Arctic and three Antarctic sites, and simulation results of two numerical models: a 2-D atmospheric chemistry model and a 1-D firn diffusion model. The first one is used to calculate atmospheric concentrations from emission trends based on industrial inventories; the calculated concentration trends are used by the second one to produce depth concentration profiles in the firn. The 2-D atmospheric model is validated in the boundary layer by comparison with atmospheric station measurements, and vertically for CFC-12 by comparison with balloon and FTIR measurements. Firn air measurements provide constraints on historical atmospheric concentrations over the last century. Age distributions in the firn are discussed using a Green function approach. Finally, our results are used as input to a radiative model in order to evaluate the radiative forcing of our target gases. Multi-species and multi-site firn air studies allow to better constrain atmospheric trends. The low concentrations of all studied gases at the bottom of the firn, and their consistency with our model results confirm that their natural sources are small. Our results indicate that the emissions, sinks and trends of CFC-11, CFC-12, CFC-113, CFC-115 and SF6 are well constrained, whereas it is not the case for CFC-114 and CCl4. Significant emission-dependent changes in the lifetimes of halocarbons destroyed in the stratosphere were obtained. Those result from the time needed for their transport from the surface where they are emitted to the stratosphere where they are destroyed. Efforts should be made to update and reduce the large uncertainties on CFC lifetimes.

Chemical and aerosol characterisation of the troposphere over West Africa during the monsoon period as part of AMMA

During June, July and August 2006 five aircraft took part in a campaign over West Africa to observe the aerosol content and chemical composition of the troposphere and lower stratosphere as part of the African Monsoon Multidisciplinary Analysis (AMMA) project. These are the first such measurements in this region during the monsoon period. In addition to providing an overview of the tropospheric composition, this paper provides a description of the measurement strategy (flights performed, instrumental payloads, wing-tip to wing-tip comparisons) and points to some of the important findings discussed in more detail in other papers in this special issue. The ozone data exhibits an "S" shaped vertical profile which appears to result from significant losses in the lower troposphere due to rapid deposition to forested areas and photochemical destruction in the moist monsoon air, and convective uplift of ozone-poor air to the upper troposphere. This profile is disturbed, particularly in the south of the region, by the intrusions in the lower and middle troposphere of air from the southern hemisphere impacted by biomass burning. Comparisons with longer term data sets suggest the impact of these intrusions on West Africa in 2006 was greater than in other recent wet seasons. There is evidence for net photochemical production of ozone in these biomass burning plumes as well as in urban plumes, in particular that from Lagos, convective outflow in the upper troposphere and in boundary layer air affected by nitrogen oxide emissions from recently wetted soils. This latter effect, along with enhanced deposition to the forested areas, contributes to a latitudinal gradient of ozone in the lower troposphere. Biogenic volatile organic compounds are also important in defining the composition both for the boundary layer and upper tropospheric convective outflow. Mineral dust was found to be the most abundant and ubiquitous aerosol type in the atmosphere over Western Africa. Data collected within AMMA indicate that injection of dust to altitudes favourable for long-range transport (i.e. in the upper Sahelian planetary boundary layer) can occur behind the leading edge of mesoscale convective system (MCS) cold-pools. Research within AMMA also provides the first estimates of secondary organic aerosols across the West African Sahel and have shown that organic mass loadings vary between 0 and 2 μg m−3 with a median concentration of 1.07 μg m−3. The vertical distribution of nucleation mode particle concentrations reveals that significant and fairly strong particle formation events did occur for a considerable fraction of measurement time above 8 km (and only there). Very low concentrations were observed in general in the fresh outflow of active MCSs, likely as the result of efficient wet removal of aerosol particles due to heavy precipitation inside the convective cells of the MCSs. This wet removal initially affects all particle size ranges as clearly shown by all measurements in the vicinity of MCSs.

Evaluation of a Lagrangian box model using field measurements from EASE (Eastern Atlantic Summer Experiment) 1996

The Cambridge Tropospheric Trajectory model of Chemistry and Transport (CiTTyCAT), a Lagrangian chemistry model, has been evaluated using atmospheric chemical measurements collected during the East Atlantic Summer Experiment 1996 (EASE '96). This field campaign was part of the UK Natural Environment Research Council's (NERC) Atmospheric Chemistry Studies in the Oceanic Environment (ACSOE) programme, conducted at Mace Head, Republic of Ireland, during July and August 1996. The model includes a description of gas-phase tropospheric chemistry, and simple parameterisations for surface deposition, mixing from the free troposphere and emissions. The model generally compares well with the measurements and is used to study the production and loss of O3 under a variety of conditions. The mean difference between the hourly O3 concentrations calculated by the model and those measured is 0.6 ppbv with a standard deviation of 8.7 ppbv. Three specific air-flow regimes were identified during the campaign – westerly, anticyclonic (easterly) and south westerly. The westerly flow is typical of background conditions for Mace Head. However, on some occasions there was evidence of long-range transport of pollutants from North America. In periods of anticyclonic flow, air parcels had collected emissions of NOx and VOCs immediately before arriving at Mace Head, leading to O3 production. The level of calculated O3 depends critically on the precise details of the trajectory, and hence on the emissions into the air parcel. In several periods of south westerly flow, low concentrations of O3 were measured which were consistent with deposition and photochemical destruction inside the tropical marine boundary layer.

The impact of finer-resolution air-sea coupling on the intraseasonal oscillation of the Indian monsoon

The new HadKPP atmosphere–ocean coupled model is described and then used to determine the effects of sub-daily air–sea coupling and fine near-surface ocean vertical resolution on the representation of the Northern Hemisphere summer intra-seasonal oscillation. HadKPP comprises the Hadley Centre atmospheric model coupled to the K Profile Parameterization ocean-boundary-layer model. Four 30-member ensembles were performed that varied in oceanic vertical resolution between 1 m and 10 m and in coupling frequency between 3 h and 24 h. The 10 m, 24 h ensemble exhibited roughly 60% of the observed 30–50 day variability in sea-surface temperatures and rainfall and very weak northward propagation. Enhancing either only the vertical resolution or only the coupling frequency produced modest improvements in variability and only a standing intra-seasonal oscillation. Only the 1 m, 3 h configuration generated organized, northward-propagating convection similar to observations. Sub-daily surface forcing produced stronger upper-ocean temperature anomalies in quadrature with anomalous convection, which likely affected lower-atmospheric stability ahead of the convection, causing propagation. Well-resolved air–sea coupling did not improve the eastward propagation of the boreal summer intra-seasonal oscillation in this model. Upper-ocean vertical mixing and diurnal variability in coupled models must be improved to accurately resolve and simulate tropical sub-seasonal variability. In HadKPP, the mere presence of air–sea coupling was not sufficient to generate an intra-seasonal oscillation resembling observations.

Moisture transport in mid-latitude cyclones

We discuss how synoptic-scale variability controls the transport of atmospheric water vapour by mid-latitude cyclones. Idealised simulations are used to investigate quantitatively what factors determine the magnitude of cyclone moisture transport. It is demonstrated that large-scale ascent on the warmconveyor belt and shallow cumulus convection are equally important for ventilating moisture from the boundary layer into the free troposphere, and that ventilated moisture can be transported large distances eastwards and polewards by the cyclone, before being returned to the surface as precipitation. The initial relative humidity is shown to have little affect on the ability of the cyclone to transport moisture, whilst the absolute temperature and meridional temperature gradient provide much stronger controls. Scaling arguments are presented to quantify the dependence of moisture transport on large-scale and boundary-layer parameters. It is shown that ventilation by shallow convection and warm-conveyor belt advection vary in the same way with changes to large-scale parameters. However, shallow convective ventilation has a much stronger dependence on boundary-layer parameters than warm-conveyor belt ventilation.

Joint modelling of obstacle induced and mesoscale changes: current limits and challenges

Obstacles considerably influence boundary layer processes. Their influences have been included in mesoscale models (MeM) for a long time. Methods used to parameterise obstacle effects in a MeM are summarised in this paper using results of the mesoscale model METRAS as examples. Besides the parameterisation of obstacle influences it is also possible to use a joint modelling approach to describe obstacle induced and mesoscale changes. Three different methods may be used for joint modelling approaches: The first method is a time-slice approach, where steady basic state profiles are used in an obstacle resolving microscale model (MiM, example model MITRAS) and diurnal cycles are derived by joining steady-state MITRAS results. The second joint modelling approach is one-way nesting, where the MeM results are used to initialise the MiM and to drive the boundary values of the MiM dependent on time. The third joint modelling approach is to apply multi-scale models or two-way nesting approaches, which include feedbacks from the MiM to the MeM. The advantages and disadvantages of the different approaches and remaining problems with joint Reynolds-averaged Navier–Stokes modelling approaches are summarised in the paper.

Forecast impact of targeted observations: sensitivity to observation error and proximity to steep orography

For a targeted observations case, the dependence of the size of the forecast impact on the targeted dropsonde observation error in the data assimilation is assessed. The targeted observations were made in the lee of Greenland; the dependence of the impact on the proximity of the observations to the Greenland coast is also investigated. Experiments were conducted using the Met Office Unified Model (MetUM), over a limited-area domain at 24-km grid spacing, with a four-dimensional variational data assimilation (4D-Var) scheme. Reducing the operational dropsonde observation errors by one-half increases the maximum forecast improvement from 5% to 7%–10%, measured in terms of total energy. However, the largest impact is seen by replacing two dropsondes on the Greenland coast with two farther from the steep orography; this increases the maximum forecast improvement from 5% to 18% for an 18-h forecast (using operational observation errors). Forecast degradation caused by two dropsonde observations on the Greenland coast is shown to arise from spreading of data by the background errors up the steep slope of Greenland. Removing boundary layer data from these dropsondes reduces the forecast degradation, but it is only a partial solution to this problem. Although only from one case study, these results suggest that observations positioned within a correlation length scale of steep orography may degrade the forecast through the anomalous upslope spreading of analysis increments along terrain-following model levels.

Initiation of deep convection at marginal instability in an ensemble of mesoscale models: a case-study from COPS

The present study investigates the initiation of precipitating deep convection in an ensemble of convection-resolving mesoscale models. Results of eight different model runs from five non-hydrostatic models are compared for a case of the Convective and Orographically-induced Precipitation Study (COPS). An isolated convective cell initiated east of the Black Forest crest in southwest Germany, although convective available potential energy was only moderate and convective inhibition was high. Measurements revealed that, due to the absence of synoptic forcing, convection was initiated by local processes related to the orography. In particular, the lifting by low-level convergence in the planetary boundary layer is assumed to be the dominant process on that day. The models used different configurations as well as different initial and boundary conditions. By comparing the different model performance with each other and with measurements, the processes which need to be well represented to initiate convection at the right place and time are discussed. Besides an accurate specification of the thermodynamic and kinematic fields, the results highlight the role of boundary-layer convergence features for quantitative precipitation forecasts in mountainous terrain.

Moisture vertical structure, column water vapor, and tropical deep convection

The vertical structure of the relationship between water vapor and precipitation is analyzed in 5 yr of radiosonde and precipitation gauge data from the Nauru Atmospheric Radiation Measurement (ARM) site. The first vertical principal component of specific humidity is very highly correlated with column water vapor (CWV) and has a maximum of both total and fractional variance captured in the lower free troposphere (around 800 hPa). Moisture profiles conditionally averaged on precipitation show a strong association between rainfall and moisture variability in the free troposphere and little boundary layer variability. A sharp pickup in precipitation occurs near a critical value of CWV, confirming satellite-based studies. A lag–lead analysis suggests it is unlikely that the increase in water vapor is just a result of the falling precipitation. To investigate mechanisms for the CWV–precipitation relationship, entraining plume buoyancy is examined in sonde data and simplified cases. For several different mixing schemes, higher CWV results in progressively greater plume buoyancies, particularly in the upper troposphere, indicating conditions favorable for deep convection. All other things being equal, higher values of lower-tropospheric humidity, via entrainment, play a major role in this buoyancy increase. A small but significant increase in subcloud layer moisture with increasing CWV also contributes to buoyancy. Entrainment coefficients inversely proportional to distance from the surface, associated with mass flux increase through a deep lower-tropospheric layer, appear promising. These yield a relatively even weighting through the lower troposphere for the contribution of environmental water vapor to midtropospheric buoyancy, explaining the association of CWV and buoyancy available for deep convection.

Simulations of the London urban heat island

We present simulations of London's meteorology using the Met Office Unified Model with a new, sophisticated surface energy-balance scheme to represent the urban surfaces, called MORUSES. Simulations are performed with the urban surfaces represented and with the urban surfaces replaced with grass in order to calculate the urban increment on the local meteorology. The local urban effects were moderated to some extent by the passage of an onshore flow that propagated up the Thames estuary and across the city, cooling London slightly in the afternoon. Validations of screen-level temperature show encouraging agreement to within 1–2 K, when the urban increment is up to 5 K. The model results are then used to examine factors shaping the spatial and temporal structure of London's atmospheric boundary layer. The simulations reconcile the differences in the temporal evolution of the urban heat island (UHI) shown in various studies and demonstrate that the variation of UHI with time depends strongly on the urban fetch. The UHI at a location downwind of the city centre shows a decrease in UHI during the night, while the UHI at the city centre stays constant. Finally, the UHI at a location upwind of the city centre increases continuously. The magnitude of the UHI by the time of the evening transition increases with urban fetch. The urban increments are largest at night, when the boundary layer is shallow. The boundary layer experiences continued warming after sunset, as the heat from the urban fabric is released, and a weakly convective boundary layer develops across the city. The urban land-use fraction is the dominant control on the spatial structure in the sensible heat flux and the resulting urban increment, although even the weak advection present in this case study is sufficient to advect the peak temperature increments downwind of the most built-up areas. Copyright © 2011 Royal Meteorological Society and British Crown Copyright, the Met Office

Kinetics of the reaction between OH radicals and monochlorodimethylsulphide (CH3SCH2Cl)

The gas-phase rate coefficient for the reaction between OH radicals and CH3SCH2Cl (MCDMS) was determined to be (2.5±1.3)×10−12 cm3 molecule−1 s−1 using the discharge–flow kinetic technique. An estimate of ≈10−10 cm3 molecule−1 s−1 was obtained for the rate coefficient for reaction of Cl with MCDMS. It would appear that the reaction with OH is not the main loss process for CH3SCH2Cl in the marine boundary layer. The possible implications for the MBL of halogen-promoted oxidation of dimethylsulphide are considered.

Conditional symmetric instability in sting-jet storms

Sting jets are transient mesoscale jets of air that descend from the tip of the cloud head towards the top of the boundary layer in severe extratropical cyclones and can lead to damaging surface wind gusts. This recently identified jet is distinct from the well-documented jets associated with the cold and warm conveyor belts. One mechanism proposed for their development is the release of conditional symmetric instability (CSI). Here the spatial distribution and temporal evolution of several CSI diagnostics in four severe storms are analysed. A sting jet has been identified in three of these storms; for comparison, we also analysed one storm that did not have a sting jet, even though it hadmany of the apparent features of sting-jet storms. The sting-jet storms are distinct from the non-sting-jet storms by having much greater andmore extensive conditional instability (CI) and CSI. CSI is released by ascending air parcels in the cloud head in two of the sting-jet storms and by descending air parcels in the other sting-jet storm. By contrast, only weak CI to ascending air parcels is present at the cloud-head tip in the non-sting-jet storm. CSI released by descending air parcels, as diagnosed by decaying downdraught slantwise convective available potential energy (DSCAPE), is collocated with the sting jets in all three sting-jet storms and has a localisedmaximum in two of them. Consistent evolutions of saturated moist potential vorticity are found.We conclude that CSI release has a role in the generation of the sting jet, that the sting jet may be driven by the release of instability to both ascending and descending parcels, and that DSCAPE could be used as a discriminating diagnostic for the sting jet based on these four case-studies.

Particle image velocimetry measurements of turbulent flow within outdoor and indoor urban scale models and flushing motions in urban canopy layers

We investigate the spatial characteristics of urban-like canopy flow by applying particle image velocimetry (PIV) to atmospheric turbulence. The study site was a Comprehensive Outdoor Scale MOdel (COSMO) experiment for urban climate in Japan. The PIV system captured the two-dimensional flow field within the canopy layer continuously for an hour with a sampling frequency of 30 Hz, thereby providing reliable outdoor turbulence statistics. PIV measurements in a wind-tunnel facility using similar roughness geometry, but with a lower sampling frequency of 4 Hz, were also done for comparison. The turbulent momentum flux from COSMO, and the wind tunnel showed similar values and distributions when scaled using friction velocity. Some different characteristics between outdoor and indoor flow fields were mainly caused by the larger fluctuations in wind direction for the atmospheric turbulence. The focus of the analysis is on a variety of instantaneous turbulent flow structures. One remarkable flow structure is termed 'flushing', that is, a large-scale upward motion prevailing across the whole vertical cross-section of a building gap. This is observed intermittently, whereby tracer particles are flushed vertically out from the canopy layer. Flushing phenomena are also observed in the wind tunnel where there is neither thermal stratification nor outer-layer turbulence. It is suggested that flushing phenomena are correlated with the passing of large-scale low-momentum regions above the canopy.

Global retrieval of ATSR cloud parameters and evaluation (GRAPE): dataset assessment

The Along-Track Scanning Radiometers (ATSRs) provide a long time-series of measurements suitable for the retrieval of cloud properties. This work evaluates the freely-available Global Retrieval of ATSR Cloud Parameters and Evaluation (GRAPE) dataset (version 3) created from the ATSR-2 (1995�2003) and Advanced ATSR (AATSR; 2002 onwards) records. Users are recommended to consider only retrievals flagged as high-quality, where there is a good consistency between the measurements and the retrieved state (corresponding to about 60% of converged retrievals over sea, and more than 80% over land). Cloud properties are found to be generally free of any significant spurious trends relating to satellite zenith angle. Estimates of the random error on retrieved cloud properties are suggested to be generally appropriate for optically-thick clouds, and up to a factor of two too small for optically-thin cases. The correspondence between ATSR-2 and AATSR cloud properties is high, but a relative calibration difference between the sensors of order 5�10% at 660 nm and 870 nm limits the potential of the current version of the dataset for trend analysis. As ATSR-2 is thought to have the better absolute calibration, the discussion focusses on this portion of the record. Cloud-top heights from GRAPE compare well to ground-based data at four sites, particularly for shallow clouds. Clouds forming in boundary-layer inversions are typically around 1 km too high in GRAPE due to poorly-resolved inversions in the modelled temperature profiles used. Global cloud fields are compared to satellite products derived from the Moderate Resolution Imaging Spectroradiometer (MODIS), Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) measurements, and a climatology of liquid water content derived from satellite microwave radiometers. In all cases the main reasons for differences are linked to differing sensitivity to, and treatment of, multi-layer cloud systems. The correlation coefficient between GRAPE and the two MODIS products considered is generally high (greater than 0.7 for most cloud properties), except for liquid and ice cloud effective radius, which also show biases between the datasets. For liquid clouds, part of the difference is linked to choice of wavelengths used in the retrieval. Total cloud cover is slightly lower in GRAPE (0.64) than the CALIOP dataset (0.66). GRAPE underestimates liquid cloud water path relative to microwave radiometers by up to 100 g m�2 near the Equator and overestimates by around 50 g m�2 in the storm tracks. Finally, potential future improvements to the algorithm are outlined.